NDLI: Cobalt-Catalyzed Hydrogenation Reactions Enabled by Ligand-Based Storage of Dihydrogen.

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Cobalt-Catalyzed Hydrogenation Reactions Enabled by Ligand-Based Storage of Dihydrogen.

Content Provider	Europe PMC
Author	Anferov, SophieW. Filatov, Alexander S. Anderson, John S.
Copyright Year	2022
Abstract	The use of supporting ligands that can store either protonsorelectrons has emerged as a powerful strategy in catalysis. While thesestrategies are potent individually, natural systems mediate remarkabletransformations by combining the storage of both protons and electronsin the secondary coordination sphere. As such, there has been recentinterest in using this strategy to enable fundamentally differenttransformations. Furthermore, outsourcing H-atom or hydrogen storageto ancillary ligands can also enable alternative mechanistic pathwaysand thereby selectivity. Here, we describe the application of thisstrategy to facilitate radical reactivity in Co-based hydrogenationcatalysis. Metalation of previously reported dihydrazonopyrrole ligandswith Co results in paramagnetic complexes, which are best describedas having Co(II) oxidation states. These complexes catalytically hydrogenateolefins with low catalyst loadings under mild conditions (1 atm H2, 23 °C). Mechanistic, spectroscopic, and computationalinvestigations indicate that this system goes through a radical hydrogen-atomtransfer (HAT) type pathway that is distinct from classic organometallicmechanisms and is supported by the ability of the ligand to storeH2. These results show how ancillary ligands can facilitateefficient catalysis, and furthermore how classic organometallic mechanismsfor catalysis can be altered by the secondary coordination sphere.
Related Links	https://europepmc.org/backend/ptpmcrender.fcgi?accid=PMC9396622&blobtype=pdf
Journal	ACS Catalysis [ACS Catal]
Volume Number	12
DOI	10.1021/acscatal.2c02467
PubMed Central reference number	PMC9396622
Issue Number	16
PubMed reference number	36033368
e-ISSN	21555435
Language	English
Publisher	American Chemical Society
Publisher Date	2022-08-01
Access Restriction	Open
Rights License	Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). © 2022 The Authors. Published by American Chemical Society
Subject Keyword	catalysis redox-active cobalt hydrogenation hydrogen
Content Type	Text
Resource Type	Article
Subject	Chemistry Catalysis

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